In recent few years, significant improvement has been made in developing largescale 3D printers to accommodate the need of industrial-scale 3D printing. It is of great feasibility to construct structural components and buildings by means of 3D concrete printing. The major issues of this innovative technique focus on the preparation and optimization of concrete materials which possess favourable printable properties as well as the measurement and evaluation methods of their workability. This paper firstly introduces three largescale 3D printing systems that have been successfully applied in construction industry. It then summarizes the commonly used raw materials in concrete manufacturing. Critical factors that should be particularly controlled in material preparation are specified. Easy-extrusive, easy-flowing, well-buildable, proper setting time and low shrinkage are significant for concrete mixture to meet the critical requirements of a freeform construction process. Thereafter, measuring methods that can be employed to assess the fresh and hardened properties of concrete at early stages are suggested. Finally, a few of evaluation methods are presented which may offer certain assistance for optimizing material preparation. The objective of this work is to review current design methodologies and experimental measurement and evaluation methods for 3D printable concrete materials and promote its responsible use with largescale 3D printing technology.